The influence of hyperchaoticity, synchronization, and Shannon entropy on the performance of a physical reservoir computer.

In this paper, we analyze the dynamic effect of a reservoir computer (RC) on its performance. Modified Kuramoto's coupled oscillators are used to model the RC, and synchronization, Lyapunov spectrum (and dimension), Shannon entropy, and the upper bound of the Kolmogorov-Sinai entropy are employed to characterize the dynamics of the RC. The performance of the RC is analyzed by reproducing the distribution of random, Gaussian, and quantum jumps series (shelved states) since a replica of the time evolution of a completely random series is not possible to generate. We demonstrate that hyperchaotic motion, moderate Shannon entropy, and a higher degree of synchronization of Kuramoto's oscillators lead to the best performance of the RC. Therefore, an appropriate balance of irregularity and order in the oscillator's dynamics leads to better performances.

Local excitation and valley polarization in graphene with multi-harmonic pulses.

We elucidate the mechanism of strong laser pulse excitation in pristine graphene with multi-harmonic pulses, linearly polarized parallel to the line connecting the two different Dirac points in the Brillouin zone and with a maximal vector potential given by the distance of those points. The latter two conditions have emerged from our previous work [Kelardeh et al., Phys. Rev. Res., 2022, 4, L022014] as favorable for large valley polarization. We introduce a novel compacted representation for excitation, locally resolved in the initial conditions for the crystal momenta. These maps are our main tool to gain insight into the excitation dynamics. They also help with understanding the effect of dephasing. We work out why a long wavelength and a moderate number of overtones in the harmonic pulse generate the largest valley polarizations.

Decoherence-Induced Universality in Simple Metal Cluster Photoelectron Angular Distributions.

Measured angular distributions of photoelectrons from size-selected copper and sodium cluster anions are demonstrated to exhibit a universal behavior independent of the initial electron state, cluster size, or material, which can be traced back to momentum conservation upon photoemission. Quantum simulations reproduce the universality under the assumption that multielectron dynamics localizes the emission on the cluster surface and renders the cluster opaque to photoelectrons, thereby quenching interference effects that would otherwise obscure this almost classical behavior.

Perspectives for analyzing non-linear photo-ionization spectra with deep neural networks trained with synthetic Hamilton matrices.

We have constructed deep neural networks, which can map fluctuating photo-electron spectra obtained from noisy pulses to spectra from noise-free pulses. The network is trained on spectra from noisy pulses in combination with random Hamilton matrices, representing systems which could exist but do not necessarily exist. In [Giri et al., Phys. Rev. Lett., 2020, 124, 113201] we performed a purification of fluctuating spectra, that is, mapping them to those from Fourier-limited Gaussian pulses. Here, we investigate the performance of such neural-network-based maps for predicting spectra of double pulses, pulses with a chirp and even partially-coherent pulses from fluctuating spectra generated by noisy pulses. Secondly, we demonstrate that along with purification of a fluctuating double-pulse spectrum, one can estimate the time-delay of the underlying double pulse, an attractive feature for single-shot spectra from SASE FELs. We demonstrate our approach with resonant two-photon ionization, a non-linear process, sensitive to details of the laser pulse.

Nonadiabatic Molecular Association in Thermal Gases Driven by Radio-Frequency Pulses.

The molecular association process in a thermal gas of ^{85}Rb is investigated where the effects of the envelope of the radio-frequency field are taken into account. For experimentally relevant parameters our analysis shows that with increasing pulse length the corresponding molecular conversion efficiency exhibits low-frequency interference fringes which are robust under thermal averaging over a wide range of temperatures. This dynamical interference phenomenon is attributed to Stückelberg phase accumulation between the low-energy continuum states and the dressed molecular state which exhibits a shift proportional to the envelope of the radio-frequency pulse intensity.

Deformation of Atomic p_{±} Orbitals in Strong Elliptically Polarized Laser Fields: Ionization Time Drifts and Spatial Photoelectron Separation.

We theoretically investigate the deformation of atomic p_{±} orbitals driven by strong elliptically polarized (EP) laser fields and the role it plays in tunnel ionization. Our study reveals that different Stark effects induced by orthogonal components of the EP field give rise to subcycle rearrangement of the bound electron density, rendering the initial p_{+} and p_{-} orbitals deformed and polarized along distinctively tilted angles with respect to the polarization ellipse of the EP field. As a consequence, the instantaneous tunneling rates change such that for few-cycle EP laser pulses the bound electron initially counterrotating (corotating) with the electric field is most likely released before (after) the peak of the electric field. We demonstrate that with a sequential-pulse setup one can exploit this effect to spatially separate the photoelectrons detached from p_{+} and p_{-} orbitals, paving the way towards robust control of spin-resolved photoemission in laser-matter interactions.

Polyatomic Trilobite Rydberg Molecules in a Dense Random Gas.

Trilobites are exotic giant dimers with enormous dipole moments. They consist of a Rydberg atom and a distant ground-state atom bound together by short-range electron-neutral attraction. We show that highly polar, polyatomic trilobite states unexpectedly persist and thrive in a dense ultracold gas of randomly positioned atoms. This is caused by perturbation-induced quantum scarring and the localization of electron density on randomly occurring atom clusters. At certain densities these states also mix with an s state, overcoming selection rules that hinder the photoassociation of ordinary trilobites.

Tunneling Ionization Time Resolved by Backpropagation.

We determine the ionization time in tunneling ionization by an elliptically polarized light pulse relative to its maximum. This is achieved by a full quantum propagation of the electron wave function forward in time, followed by a classical backpropagation to identify tunneling parameters, in particular, the fraction of electrons that has tunneled out. We find that the ionization time is close to zero for single active electrons in helium and in hydrogen if the fraction of tunneled electrons is large. We expect our analysis to be essential to quantify ionization times for correlated electron motion.

Proton ejection from molecular hydride clusters exposed to strong x-ray pulses.

Clusters consisting of small molecules containing hydrogen do eject fast protons when illuminated by short x-ray pulses. A suitable overall charging of the cluster controlled by the x-ray intensity induces electron migration from the surface to the bulk leading to efficient segregation of the protons and to a globally hindered explosion of the heavy atoms even outside the screened volume. We investigate this peculiar effect systematically along the isoelectronic sequence of methane over ammonia and water to the atomic limit of neon as a reference. In contrast to core-shell systems where the outer shell is sacrificed to reduce radiation damage, the intricate proton dynamics of hydride clusters allows one to keep the entire backbone of heavy atoms intact.

Massively parallel ionization of extended atomic systems.

Massively parallel ionization of many atoms in a cluster or biomolecule is identified as a new phenomenon of light-matter interaction which becomes feasible through short and intense FEL pulses. Almost simultaneously emitted from the illuminated target the photo-electrons can have such a high density that they interact substantially even after photoionization. This interaction results in a characteristic electron spectrum which can be interpreted as a convolution of a mean-field electron dynamics and binary electron-electron collisions. We demonstrate that this universal spectrum can be obtained analytically by summing synthetic two-body Coulomb collision events. Moreover, we propose an experiment with hydrogen clusters to observe massively parallel ionization.

Suppression of exponential electronic decay in a charged environment.

Inner-shell ionization of atoms and molecules leads to the creation of highly excited ionic states that often decay by electron emission. The dynamics of the decay is usually assumed to be exponential and the process is characterized by a decay rate. Here we show that in a multiply ionized cluster created by interaction with a high-intensity free-electron laser (FEL) radiation, trapping of the emitted electron by the neighboring ions changes the character of the decay dynamics qualitatively to the extent that it can become oscillatory instead of exponential. Implications of the predicted effect on Coster-Kronig and interatomic Coulombic decay processes induced by FELs are investigated.

Small rare-gas clusters in soft x-ray pulses.

We develop a microscopic model for the interaction of small rare-gas clusters with soft x-ray radiation from a free electron laser. It is shown that, while the overall charging of the clusters is rather low, unexpectedly high atomic charge states can arise due to charge imbalances inside the cluster. These findings are explained by an increased absorption via inverse bremsstrahlung due to high intermediate charge states and by a nonhomogenous charge distribution inside the cluster.

Ionization of Clusters in Intense Laser Pulses through Collective Electron Dynamics.

The motion of electrons and ions in medium-sized rare gas clusters ( approximately 1000 atoms) exposed to intense laser pulses is studied microscopically by means of classical molecular dynamics using a hierarchical tree code. Pulse parameters for optimum ionization are found to be wavelength dependent. This resonant behavior is traced back to a collective electron oscillation inside the charged cluster. It is shown that this dynamics can be well described by a driven and damped harmonic oscillator allowing for a clear discrimination against other energy absorption mechanisms.

Ionization of clusters in strong x-ray laser pulses.

The effect of intense x-ray laser interaction on argon clusters is studied theoretically with a mixed quantum/classical approach. In comparison to a single atom we find that ionization of the cluster is suppressed, which is in striking contrast to the observed behavior of rare-gas clusters in intense optical laser pulses. We have identified two effects responsible for this phenomenon: A high space charge of the cluster in combination with a small quiver amplitude and delocalization of electrons in the cluster. We elucidate their impact for different field strengths and cluster sizes.

Separation and identification of dominant mechanisms in double photoionization.

Double photoionization by a single photon is often discussed in terms of two contributing mechanisms, knockout (two-step-one) and shakeoff, with the latter being a pure quantum effect. It is shown that a quasiclassical description of knockout and a simple quantum calculation of shakeoff provides a clear separation of the mechanisms and facilitates their calculation considerably. The relevance of each mechanism at different photon energies is quantified for helium. Photoionization ratios, integral, and singly differential cross sections obtained by us are in excellent agreement with benchmark experimental data and recent theoretical results.